High-order harmonic generation of the N2 molecule in two-color circularly polarized laser fields

The generation of high-order harmonics and the attosecond pulse of the N₂ molecule in two-color circularly polarized laser fields are investigated by the strong-field Lewenstein model. We show that the plateau of spectra is dramatically extended and a continuous harmonic spectrum with the bandwidth of 113 eV is obtained. When a static field is added to the x direction, the quantum path control is realized and a supercontinuum spectrum can be obtained, which is beneficial to obtain a shorter attosecond pulse. The underlying physical mechanism is well explained by the time-frequency analysis and the semi-classical three-step model with a finite initial transverse velocity. By superposing several orders of harmonics in the combination of two-color circularly polarized laser fields and a static field, an isolated attosecond pulse with a duration of 30 as can be generated.     

碳分子线C5在激光场中的含时密度泛函理论研究

运用含时密度泛函理论和分子动力学相结合的方法, 研究了C₅分子线在强激光场中的电离激发.研究发现, 当考虑激光强度对C₅分子线激发的影响时, 激光强度越强, 分子吸收的能量越多, 电离也越早, 最终电离的电子也越多, 而且沿激光极化方向的偶极矩的变化及峰值也越大. 关于激光极化方向对C₅分子线激发的影响的研究表明, 当激光极化方向沿着C₅分子线轴向时, 分子的电离大大增强, x方向的激光脉冲仅能激发起x方向的偶极振荡, 而y方向的激光脉冲仅能激发起y方向的偶极振荡, 而且x方向的激光脉冲激发的偶极振荡强. 研究还表明, 当激光极化方向沿着C₅分子线轴向时, 尽管由于电离增强而导致C₅分子线C–C键振动的同步性变差, 但在两种激光极化方向情况下, C₅分子线的振动模式与中性C₅分子线的振动模式相同. 关键词： 含时密度泛函理论 分子动力学 分子电离 碳分子线     

Li修饰的C$lt;sub$gt;6$lt;/sub$gt;分子对H$lt;sub$gt;2$lt;/sub$gt;O的吸附研究

采用密度泛函理论中的广义梯度近似研究C₆Li吸附H₂O分子并将之进行分解的催化过程. 几何优化发现：Li原子最稳定的吸附位置是位于C 原子顶位上方. 研究表明,第一个H₂O 分子吸附在C₆Li上需要克服1.77 eV的能量势垒,然后分解为H和OH且与Li原子成键. 当吸附第二个H₂O分子时,第二个H₂O分子需要克服1.2 eV的能量势垒分解为H和OH,其中H与Li原子上的H原子结合成H₂,OH则替代Li 原子上的H结合在Li原子上. 因此C₆Li 可以作为催化剂将H₂O分子进行分解得到H₂. 分析可知：C₆Li主要是通过Li原子与H₂O之间形成的偶极矩作用来吸附H₂O 分子,与C₆₀Li₁₂ 的储氢机制类似. 研究结果可为储氢材料的制备提供一个新的思路. 关键词： 6')" href="#">C₆ Li 2O')" href="#">H₂O 密度泛函理论     

碳硼富勒烯衍生物C18B2M(M=Li,Ti, Fe)的储氢性能计算研究

本文使用密度泛函理论(density functional theory, DFT)中的广义梯度近似(generalized gradient approximation, GGA)研究了经碱金属原子Li、过渡金属原子Ti和Fe原子修饰的富勒烯C₁₈B₂M(M=Li, Ti, Fe)的储氢性能. 研究发现, C₁₈B₂由于B的替代掺杂, 比C₂₀对金属原子具有更高的结合能. 由平均吸附能分析可知: C₁₈B₂Li对H₂的吸附能力较弱, C₁₈B₂Fe对H₂的吸附能力过强, 而C₁₈B₂Ti对H₂的平均吸附能介于0.45-0.59 eV 之间, 介于物理吸附和化学吸附之间 (0.2-0.6 eV), 因此可以实现常温下的可逆储氢. C₁₈B₂M(M=Li, Ti, Fe)能够吸附的H₂数目最多分别为4, 6和4. 由储氢机理分析可知: C₁₈B₂Li主要通过碱金属离子激发的静电场来吸附H₂, 而C₁₈B₂Ti和C₁₈B₂Fe主要通过金属原子与H₂之间的Kubas作用来吸附H₂. 由于C₁₈B₂Ti既有较大的储氢数目, 又可以实现可逆储氢, 因此有望开发成新型纳米储氢材料.     

相对论圆偏振激光与固体靶作用产生高次谐波

超短超强激光与固体靶表面等离子体相互作用可以通过高次谐波的方式产生从极紫外到软X射线波段的相干辐射,获得飞秒甚至阿秒量级的超短脉冲,可用于观测原子或分子中的电子运动等超快动力学过程.本文实验研究了相对论圆偏振飞秒激光与固体靶相互作用的高次谐波产生过程,实验结果表明,在较大入射角下,圆偏振激光也可以有效地产生高次谐波辐射.通过预脉冲控制靶表面的预等离子体密度标长,发现高次谐波的产生效率随密度标长的增加而单调下降.进一步通过二维粒子模拟程序,分析了激光的偏振以及预等离子体密度标长对高次谐波产生的影响,很好地解释了实验观测结果.     

Generation of elliptical isolated attosecond pulse from oriented H2+ in a linearly polarized laser field

We investigate the ellipticity of the high-order harmonic generation from the oriented H₂⁺ exposed to a linearly polarized laser field by numerically solving the two-dimensional time-dependent Schrödinger equation (2D TDSE). Numerical simulations show that the harmonic ellipticity is remarkably sensitive to the alignment angle. The harmonic spectrum is highly elliptically polarized at a specific alignment angle θ=30°, which is insensitive to the variation of the laser parameters. The position of the harmonic intensity minima indicates the high ellipticity, which can be attributed to the two-center interference effect. The high ellipticity can be explained by the phase difference of the harmonics. This result facilitates the synthesis of a highly elliptical isolated attosecond pulse with duration down to 65 as, which can be served as a powerful tool to explore the ultrafast dynamics of molecules and study chiral light-matter interaction.     

Wakefield generation by elliptically polarized femtosecond laserpulse in ionizing gases

Wakefield generation by a femtosecond laser pulse is described in the frame of the slowly varying amplitudes approximation. The amplitude of the wakefield A, is studied as a function of laser pulse and background gas parameters, and is compared with well-known results for preformed, completely ionized plasma A_p,i. It is found that the ionization processes can increase A_p as compared to A_p,i at comparatively high laser peak intensities. It is shown that the increase of the wakefield amplitude due to gas ionization is more pronounced for circularly polarized laser pulses than for linearly polarized laser pulses. The strongest enhancement of A_p in comparison with A_p,i takes place for longer laser pulses with a duration in excess of the plasma wave period when the resonant conditions for ponderomotive excitation of the wakefield are not matched. Thus, ionization processes can expand the region of parameters for efficient generation of the laser wakefields     

圆偏振激光附加太赫兹场作用下的高次谐波发射和孤立阿秒脉冲的产生

本文通过数值求解二维含时薛定谔方程,研究了圆偏振激光和太赫兹组合场作用下,H+2的高次谐波发射和孤立阿秒(1 as=10-18s)脉冲的产生.研究发现,无论在圆偏振激光场的x或y方向附加一个太赫兹场,都可以产生一个比较平滑的连续谐波谱.通过时频分析我们发现,高次谐波的贡献主要来自于短轨道.适当选取一些级次的连续谐波进行叠加,可以得到129 as或83 as的孤立阿秒脉冲.     

圆偏振激光附加太赫兹场作用下的高次谐波发射和孤立阿秒脉冲的产生

本文通过数值求解二维含时薛定谔方程,研究了圆偏振激光和太赫兹组合场作用下,H2+的高次谐波发射和孤立阿秒脉冲的产生。研究发现,无论在圆偏振激光场的 或 方向附加一个太赫兹场,都可以产生一个比较平滑的连续谐波谱。通过时频分析我们发现,高次谐波的贡献主要来自于短轨道。适当选取一些级次的连续谐波进行叠加,可以得到129 as或83 as的孤立阿秒脉冲。     

双色反向旋转圆偏振激光场下氩原子高次谐波的产生

通过二阶分裂算符法数值求解了二维含时薛定谔方程,研究了双色反向旋转圆偏振激光场作用下氩原子的高次谐波的产生.研究表明,双色反向旋转圆偏振激光场的幅值比对高次谐波发射的效率有较大影响,当幅值比为1.4时高次谐波的发射效率最高,并应用时频分析方法、经典三步模型以及利萨茹图形等解释了高次谐波发射的物理机制.研究了不同幅值比情况下谐波场的旋转偏振特性,发现对不同频段的谐波谱的电场进行叠加,谐波场的偏振特性随幅值比的不同而发生变化,但谐波场的旋向性与入射激光脉冲的旋向性相同,不受幅值比变化的影响.     

Li修饰的C24团簇的储氢性能

利用密度泛函理论研究了Li原子修饰的C₂₄团簇的储氢性能. Li原子在C₂₄团簇表面的最佳结合位是五元环. Li原子与C₂₄团簇之间的作用强于Li原子之间的相互作用, 能阻止它们在团簇表面发生聚集. 当Li原子结合到C₂₄表面时, 它们向C原子转移电子后带正电荷. 当氢分子接近这些Li原子时, 在电场作用下发生极化, 通过静电相互作用吸附在Li原子周围. 在Li修饰的C₂₄复合物中, 每个Li原子能吸附两到三个氢分子, 平均吸附能处于0.08到0.13 eV/H₂范围内. C₂₄Li₆能吸附12个氢分子, 储氢密度达到6.8 wt%.     

Minimum structure of high-harmonic spectrafrom aligned O2 and N2 molecules

We experimentally investigated the high-order harmonic generation (HHG) from aligned O₂ and N₂ molecules in a linearly polarized laser field, and presented the dependence of the harmonic spectrum on the driving laser intensity and molecular alignment angle. The minimum position of HHG of O₂ varies with changing the laser intensity, which is caused by multi-orbital interference. However, the location of the observed minimum structure in N₂ harmonic spectrum remained unchanged upon changing the laser intensity. The mechanism of the spectral minimum for N₂ case is regarded as a Cooper-like minimum in HHG associated with the molecular electronic structure. This work indicates that harmonic spectroscopy can effectively uncover information about molecular structure and electron dynamics.     

温度对飞秒激光脉冲在NaCl溶液中成丝产生的超连续谱的影响

利用飞秒激光脉冲在NaCl溶液中成丝,研究了溶液温度对飞秒激光成丝过程中产生的超连续谱的影响.发现在激光脉冲能量较低时,溶液温度对超连续谱的影响几乎可以忽略;而在激光脉冲能量较高时,随着NaCl溶液温度的升高,超连续谱呈现出被压缩的趋势.此外,在激光脉冲能量较高的情况下, NaCl中会产生大量的气泡.通过分析,得出了飞秒激光在溶液中成丝产生的气泡是影响超连续谱发射的主要因素.     

Laser phase effect on asymmetric harmonic distribution in H_2~+

The laser phase effect on the spatial distribution of the molecular high-order harmonic generation(MHHG) spectrum from H_2~+ is theoretically investigated through solving the Non-Bohn-Oppenheimer(NBO) time-dependent Schrodinger equation(TDSE).The results are shown as follows,(i) The generated harmonics from the two nuclei each present an asymmetric distribution.Particularly,when the laser phases are chosen from 0.0π to 0.6π and from 1.7π to 2.0π,the contribution from the negative-H plays a main role in harmonic generation.When the laser phases are chosen from 0.7πto 1.6k,the contribution from the positive-H to the harmonic generation is remarkably enhanced and becomes greater than that from the negative-H.The electron localization,the time-frequency analyses of the harmonic spectrum and the time-dependent wave function are shown to explain the asymmetric harmonic distribution in H_2~+,which provides us with a method to control the electron motion in molecules,(ⅱ) As the pulse duration increases,the asymmetric distributions of the MHHG in two H nuclei decrease,(ⅲ) Isotope investigation shows that the asymmetric harmonic distribution can be reduced by introducing the heavy nucleus(i.e.,D_2~+).     

超短脉冲激光烧蚀石墨产生的喷射物的时间分辨发射光谱研究

本文使用不同激光能流(18 J/cm²–115 J/cm²)和脉冲宽度(50 fs–4 ps)的超短脉冲激光在真空中(4×10^-4 Pa)烧蚀高定向热解石墨. 通过测量烧蚀喷射物的时间分辨发射光谱研究喷射物的超快时间演化. 在喷射物发射光谱中, 观察到了C₂基团的天鹅带光谱系统, 416 nm附近C₁₅基团的由电子能级¹Σ_u⁺ 和¹Σ_g⁺之间的振动跃迁产生的光谱峰以及连续谱. 50 fs, 115 J/cm²的脉冲激光烧蚀产生的喷射物的连续谱的强度衰减分为快速下降和慢速下降两个阶段(以20 ns时间延迟为分界). 这表明连续谱是由两种不同的组分贡献的. 快速下降阶段, 连续谱主要由碳等离子体通过韧致辐射产生; 慢速下降阶段, 连续谱主要由烧蚀后期产生的大颗粒碳簇的热辐射贡献. 实验结果还揭示了激光能流的提高, 会明显增加喷射物中碳等离子体和激发态C₂的含量, 但对质量稍大的C₁₅的影响较小; 此外, 50 fs脉冲激光烧蚀产生的连续谱的存在时间会随着激光能流的减小而增大, 这说明低能流更有利于在烧蚀后期产生碳簇. 脉宽主要影响喷射物连续谱的时间演化. 4 ps脉冲激光烧蚀产生的连续谱的整个时间演化过程明显慢于50 fs脉冲产生的连续谱.     

Extreme-ultraviolet harmonic generation near 13 nm with a two-color elliptically polarized laser field

Theoretical results for high-harmonic generation by a two-color elliptically polarized laser field are presented. Special emphasis is placed on coherent radiation near 13 nm in connection with the development of extreme-ultraviolet lithography. Linearly polarized radiation at this wavelength can be obtained with a linearly polarized bichromatic laser field, whereas circularly polarized radiation can be generated with a bichromatic circularly polarized field with counterrotating coplanar components. In both cases the harmonic emission efficiencies at the saturation intensity are more than 1 order of magnitude larger than for harmonic generation with a monochromatic linearly polarized field.     

DFT study of dihydrogen interactions with lithium containing organic complexes C4H4-mLim and C5H5-mLim （m = 1, 2）

The interactions of dihydrogen with lithium containing organic complexes C₄H_4-mLi_m and C₅H_5-mLi_m (m = 1, 2) were studied by means of density functional theory (DFT) calculation. For all the complexes considered, each bonded lithium atom can adsorb up to five H₂ molecules with the mean binding energy of 0.59 eV/H₂ molecule. The interactions can be attributed to the charge transfer from the H₂ bonding orbitals to the Li 2s orbitals. The kinetic stability of these hydrogen-covered organolithium molecules is discussed in terms of the energy gap between the highest occupied molecular orbital (HOMO) and lowest unoccupied molecular orbital (LUMO). The results indicate that these organiclithium structures can perhaps be used as building units for potential hydrogen storage materials.     

Controlling the contributions to high-order harmonic generation from different nuclei of N_2 with an orthogonally polarized two-color laser field

The generation of high-order harmonic and the attosecond pulse of the N2 molecule with an orthogonally polarized two-color laser field are investigated by the strong-field Lewenstein model.We show that the control of contributions to high-order harmonic generation(HHG) from different nuclei is realized by properly selecting the relative phase.When the relative phase is chosen to be φ= 0.4π,the contribution to HHG from one nucleus is much more than that from another.Interference between two nuclei can be suppressed greatly; a supercontinuum spectrum of HHG appears from 40 e V to125 e V.The underlying physical mechanism is well explained by the time–frequency analysis and the semi-classical threestep model with a finite initial transverse velocity.By superposing several orders of harmonics,an isolated attosecond pulse with a duration of 80 as can be generated.     

Multifrequency Raman generation in liquid carbon tetrachloride with two-color pumping

The multifrequency parametric Raman generation was carried out in liquid CCl₄ by using the second harmonic of a 30 ps pulsed Nd:YAG laser and its first Stokes in CCl₄ as two-color pumping. Up to 80% energy conversion efficiency of the 50 μJ pump pulse into 10 Raman components covering spectral range from 490 to 640 nm was achieved. A scheme for a multifrequency parametric Raman laser operating with pulse repetition rates up to 0.1 MHz is suggested.     

Single Ultrashort Attosecond Pulse Generation via Combination of Chirped Fundamental Laser and an Ultraviolet Controlling Pulse

We theoretically study the high-order harmonic generation (HHG) from a hydrogen atom in an intense few-cycle chirped fundamental laser in combination with an ultraviolet (uv) controlling pulse.The high-order harmonic spectrum is calculated by solving the time-dependent Schr¨odinger equation using the split-operator method.In our calculation,we present the difference of the high-order harmonic spectrum from one-dimensional (1D) model hydrogen atom and three-dimensional (3D) real hydrogen atom.We found that the plateau of the high-order harmonic generation from the 1D case and 3D case are all extended effectively to I p + 35U p due to the presence of the chirped laser pulse and the HHG supercontinuum spectrum is generated by adding an ultraviolet controlling pulse at a proper time,but the efficiency of the HHG for 3D case is more higher at the near cut-off region than the 1D case.Therefore,the generation of the attosecond pulse by synthesizing the harmonics near cut-off region have some slight differences between 1D and 3D simulations.As a real 3D case study,we show that an isolated 18 as pulse with a bandwidth of 232.5 eV is generated directly by optmizing the combination laser fields.